Pakharukova Vera P, Potemkin Dmitriy I, Rogozhnikov Vladimir N, Stonkus Olga A, Gorlova Anna M, Nikitina Nadezhda A, Suprun Evgeniy A, Brayko Andrey S, Rogov Vladimir A, Snytnikov Pavel V
Boreskov Institute of Catalysis SB RAS, Pr. Lavrentieva 5, 630090 Novosibirsk, Russia.
Department of Natural Sciences, Novosibirsk State University, Pirogova Street 2, 630090 Novosibirsk, Russia.
Nanomaterials (Basel). 2022 Sep 15;12(18):3207. doi: 10.3390/nano12183207.
CeZrO oxides (x = 0.1, 0.25, 0.5) prepared via the Pechini route were investigated using XRD analysis, N physisorption, TEM, and TPR in combination with density functional theory calculations. The Ni/CeZrO catalysts were characterized via XRD analysis, SEM-EDX, TEM-EDX, and CO chemisorption and tested in carbon dioxide methanation. The obtained CeZrO materials were single-phase solid solutions. The increase in Zr content intensified crystal structure strains and favored the reducibility of the CeZrO oxides but strongly affected their microstructure. The catalytic activity of the Ni/CeZrO catalysts was found to depend on the composition of the CeZrO supports. The detected negative effect of Zr content on the catalytic activity was attributed to the decrease in the dispersion of the Ni nanoparticles and the length of metal-support contacts due to the worsening microstructure of CeZrO oxides. The improvement of the redox properties of the CeZrO oxide supports through cation modification can be negated by changes in their microstructure and textural characteristics.
通过佩琴尼法制备的CeZrO氧化物（x = 0.1、0.25、0.5）采用X射线衍射分析、N物理吸附、透射电子显微镜和程序升温还原，并结合密度泛函理论计算进行了研究。通过X射线衍射分析、扫描电子显微镜-能谱分析、透射电子显微镜-能谱分析和一氧化碳化学吸附对Ni/CeZrO催化剂进行了表征，并在二氧化碳甲烷化反应中进行了测试。所制备的CeZrO材料为单相固溶体。Zr含量的增加加剧了晶体结构应变，有利于CeZrO氧化物的还原，但对其微观结构有很大影响。发现Ni/CeZrO催化剂的催化活性取决于CeZrO载体的组成。检测到的Zr含量对催化活性的负面影响归因于CeZrO氧化物微观结构恶化导致Ni纳米颗粒分散度降低以及金属-载体接触长度减小。CeZrO氧化物载体通过阳离子改性改善的氧化还原性能可能会因其微观结构和织构特性的变化而被抵消。
